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IONIC POLYMERS BASED ON POLYSACCHARIDES: CORRELATIONS BETWEEN STRUCTURE, PHYSICO-CHEMICAL PROPERTIES AND INTERACTION WITH OPPOSITELY CHARGED PARTICLE
Project status: Ongoing
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     In the first stage of the project "Synthesis and characterization of polyelectrolytes based on polysaccharides with different chain flexibility (Pul, Chit, Dex, Cel) in soluble or hydrogel form and studies of aggregation/adsorption of inorganic and organic particles in aqueous and non-aqueous dispersion medium” were addressed several strategies for the synthesis of ionic, soluble and crosslinked polymers (hydrogels), based on polysaccharides, able of interacting with inorganic and organic particles, dispersed in model suspensions/emulsions. In order to achieve the objectives of this stage, the following activities were carried out: 1.1. Synthesis and characterization of the chemical composition of soluble PEs (polysaccharides with cationic grafts); 1.2. Preparation and physico-chemical characterization of hydrogels in the form of monolith and/or membranes based on Chit, Pul, DxS by cryogelification technique; 1.3. aggregation of inorganic particles (zirconium silicate, clays, etc.) in aqueous/non-aqueous dispersion medium; 1.4. Adsorption of one-component pesticides by hydrogels by the freezing technique, the results of which are presented as follows:

  • Samples of soluble cationic polysaccharides based on pullulan with tertiary or quaternary ammonium amine groups with or without hydrophobic groups were synthesized and characterized (elemental analysis, 1H- and 13C-NMR spectroscopy, IR). The synthesis conditions (molar ratio between reaction partners, temperature, duration) were adapted to each type of macromolecular compound so as to obtain polyelectrolytes with a well-defined structure;
  • Samples containing tertiary amine groups or quaternary ammonium groups were selected for aggregation of inorganic particles (zirconium silicate (kreutzonite), clays, TiO2, etc.) in aqueous (different pHs) and aqueous/non-aqueous (water/methanol (%): 90/10 and 50/50) dispersion medium;
  • All investigated inorganic particles were successfully aggregated and removed (more than 95%) by Pg-pAPTAC2 and DMAPA0.16-P polymers from dispersions prepared with water regardless of the pH or water / methanol composition (%, v / v): 90/10 and 50/50; optimal polymer doses ranged from 0.4 mg L-1 to 1.4 mg L-1.

     Novel porous hydrogels were prepared by cryogelation technique and characterized (FT-IR, NMR, and SEM):

  • Porous hydrogels based on Chit and oxidized CMC (CMCox), as membranes were prepared using different molar ratios between -NH2 groups of Chit and -CHO groups of CMCox.
  • Physically cross-linked hydrogels based on Chit and DxS were designed by varying the molar ratio between -NH2 groups of Chit and -SO3Na groups of DxS, the molar mass of DxS, and the gel preparation temperature.
  • Chit-based porous hydrogels, as monoliths were obtained by combining cryogelation with porogen leaching methodology. These hydrogels have been successfully used to remove Fastac 10 EC insecticide from aqueous solutions.
  • Macroporous interpenetrating hydrogel networks based on PHEMA and Pul were also successfully synthesized.

     Samples of cationic polymers based on polysaccharides, soluble or in gel form, synthesized and tested in the aggregation and sorption experiments in the first stage of the project proved to be highly effective in reducing (90-95%) the inorganic contaminants (kreutzonite, TiO2, kaolin) and organic (complex formulation of pyrethroid insecticide-Fastac 10 EC) investigated, thus expanding the range of biodegradable, non-toxic and cheap ionic materials with potential applications in the field of wastewater purification from the ceramic and pesticides industries as well as in agriculture.

All the objectives proposed for 2021 have been fully met, the results obtained being disseminated as follows: 

Published articles 

1.Efficacy of quaternary ammonium groups based polyelectrolytes for the reduction of various pesticide formulations content from synthetic wastewater, L. Ghimici, M. Nichifor, Sep. Purif. Technol. 276 (2021) 119325. https://doi.org/10.1016/j.seppur.2021.119325 (Q1, FI= 7.312)

2. Synthesis of Thiourea-Graft-Polyethyleneimine and Its Performance in Flocculation of Some Inorganic Particles,  C.-A. Ghiorghita, L. Ghimici, G.-L. Ailiesei,  Ind. Eng. Chem. Res. 60 (14) (2021) 5167–5175. https://doi.org/10.1021/acs.iecr.1c00555, (Q2,FI= 3, 72)

3. Physically cross-linked chitosan/dextrin cryogels entrapping Thymus vulgaris essential oil with enhanced mechanical, antioxidant and antifungal properties, M. V. Dinu, A.C. Grădinaru, M. M. Lazăr, I. A. Dinu, I. E. Răschip, N. Ciocarlan -. International Journal of Biological Macromolecules 184 (2021) 898–908. https://doi.org/10.1016/j.ijbiomac.2021.06.068 (Q1, FI = 6.953)

4. Analysis of copper(II), cobalt(II) and iron(III) sorption in binary and ternary systems by chitosan-based composite sponges obtained by ice-segregation approach, Maria Valentina Dinu, Doina Humelnicu, Maria Marinela Lazăr, Gels 7 (2021) 103. https://doi.org/10.3390/gels7030103 (Q1, FI = 4.702)

Accepted articles

1. The separation of kreutzonit particles by cationic pullulan derivatives from model suspension, L. Ghimici, M. Constantin, ENVC., 5 (2021) 100352. https://doi.org/10.1016/j.envc.2021.100352

Communications

1. Aqueous Solutions of chitosan: viscometric and flocculation properties, Cristina Eliza Brunchi, L. Ghimici, Proceceeding of the 10th International Conference TEXTEH  Bucharest, Romania 2021, p. 123-129. DOI: 10.35530/TT.2021.21

2.Cryogenically-structured composite biomaterials, M.V. Dinu, M.M. Lazăr, I.E.Răschip, Congresul Internațional „Pregătim viitorul promovând excelența”, Universitatea „Apollonia” din Iași, 1-3 march 2021.

3. Chitosan aqueous solutions: viscometric and flocculation properties, C.-E.  Brunchi, L.Ghimici,  The 10th International Conference TEXTEH 2021, Bucharest, Romania October 21-22, 2021.         2. 4. 4. Formation of 1D-oriented structure in chitosan-based hydrogels, M.M. Lazăr, M.V.Dinu, Congresul Internațional „Pregătim viitorul promovând excelența”, Universitatea „Apollonia” din Iași, 1-3 march 2021.

5. 3D anisotropic polysaccharide-based cryogels as multifunctional eco-friendly materials for wastewater treatment, M.V. Dinu, M.M. Lazar, I.A. Dinu, I.E. Raschip, C.-A. Ghiorghita, L. Ghimici, 11th International Conference on Environmental Engineering and Management (ICEEM11), Muttenz, Switzerland, 8–10 September 2021.

6. Synthesis and flocculation performance of thiourea-g-polyethyleneimine, C.-A. Ghiorghita,  L. Ghimici, Congresul Internațional „Pregătim viitorul promovând excelența” , Universitatea „Apollonia” Iași, 1-3 march 2021-Poster.

 

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